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Greatly increased levels of ultraviolet (UV) radiation were observed at thirteen Arctic and sub-Arctic ground stations in the spring of 2011, when the ozone abundance in the Arctic stratosphere dropped to the lowest amounts on record. Measurements of the noontime UV Index (UVI) during the low-ozone episode exceeded the climatological mean by up to 77% at locations in the western Arctic (Alaska, Canada, Greenland) and by up to 161% in Scandinavia. The UVI measured at the end of March at the Scandinavian sites was comparable to that typically observed 15–60 days later in the year when solar elevations are much higher. The cumulative UV dose measured during the period of the ozone anomaly exceeded the climatological mean by more than two standard deviations at 11 sites. Enhancements beyond three standard deviations were observed at seven sites and increases beyond four standard deviations at two sites. At the western sites, the episode occurred in March, when the Sun was still low in the sky, limiting absolute UVI anomalies to less than 0.5 UVI units. At the Scandinavian sites, absolute UVI anomalies ranged between 1.0 and 2.2 UVI units. For example, at Finse, Norway, the noontime UVI on 30 March was 4.7, while the climatological UVI is 2.5. Although a UVI of 4.7 is still considered moderate, UV levels of this amount can lead to sunburn and photokeratitis during outdoor activity when radiation is reflected upward by snow towards the face of a person or animal. At the western sites, UV anomalies can be well explained with ozone anomalies of up to 41% below the climatological mean. At the Scandinavian sites, low ozone can only explain a UVI increase of 50–60%. The remaining enhancement was mainly caused by the absence of clouds during the low-ozone period.
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The effect of aerosol water uptake on the aerosol particle light scattering coefficient (σ<sub>sp</sub>) is described in this study by comparing measurements from five European sites: the Jungfraujoch, located in the Swiss Alps at 3580 m a.s.l.; Ny-Ålesund, located on Spitsbergen in the Arctic; Mace Head, a coastal site in Ireland; Cabauw, a rural site in the Netherlands; and Melpitz, a regional background site in Eastern Germany. These sites were selected according to the aerosol type usually encountered at that location. The scattering enhancement factor <i>f</i>(RH, λ) is the key parameter to describe the effect of water uptake on the particle light scattering. It is defined as the σ<sub>sp</sub>(RH) at a certain relative humidity (RH) and wavelength λ divided by its dry value. <i>f</i>(RH) at the five sites varied widely, starting at very low values of <i>f</i>(RH = 85%, λ = 550 nm) around 1.28 for mineral dust, and reaching up to 3.41 for Arctic aerosol. Hysteresis behavior was observed at all sites except at the Jungfraujoch (due to the absence of sea salt). Closure studies and Mie simulations showed that both size and chemical composition determine the magnitude of <i>f</i>(RH). Both parameters are also needed to successfully predict <i>f</i>(RH). Finally, the measurement results were compared to the widely used aerosol model, OPAC (Hess et al., 1998). Significant discrepancies were seen, especially at intermediate RH ranges; these were mainly attributed to inappropriate implementation of hygroscopic growth in the OPAC model. Replacement of the hygroscopic growth with values from the recent literature resulted in a clear improvement of the OPAC model.
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The zonal mean transport of ozone and carbon monoxide (CO) near the tropical tropopause is investigated using the Whole-Atmosphere Community Climate Model version 4 (WACCM4). The variability in temperature, ozone and CO in the model shows good agreement with satellite and balloon observations. Modeled temperature and tracers exhibit large and closely coupled annual cycles in the tropical lower stratosphere, as in the observations. The thermodynamic and tracer budgets in the model are analyzed based on the Transformed Eulerian Mean (TEM) framework on log-pressure coordinates and also using the isentropic formulation. Results show that the coupled seasonal cycles are mainly forced by tropical upwelling over altitudes with large vertical tracer gradients, in agreement with previous observational studies. The model also allows explicit calculation of eddy transport terms, which make an important contribution to ozone tendencies in the tropical lower stratosphere. The character of the eddy fluxes changes with altitude. At higher levels (~2 km above the cold point tropopause), isentropic eddy transport occurs during winter and spring in each hemisphere in the sub-tropics, associated with transient Rossby waves acting on strong background latitudinal gradients. At lower altitudes, close to the tropical tropopause, there is a maximum in horizontal eddy transport during boreal summer associated with the Asian monsoon anticyclone. Sub-seasonal variability in ozone and CO, tied to fluctuations in temperature, is primarily driven by transient tropical upwelling. In isentropic coordinates, the overall tracer budgets are similar to the log-pressure results, highlighting cross-isentropic advection as the main term in the time-mean balance, with large seasonality above the tropopause. However, in isentropic coordinates the tracer variability is largely reduced on both seasonal and sub-seasonal timescales, because tracer fluctuations are highly correlated with temperature (as a response to upwelling).
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Meteorological conditions may drive relationships between aerosol and cloud-related properties. It is important to account for the meteorological contribution to observed cloud–aerosol relationships in order to improve understanding of aerosol–cloud–climate interactions. A new method of investigating the contribution of meteorological covariation to observed cloud–aerosol relationships is introduced. Other studies have investigated the contribution of local meteorology to cloud–aerosol relationships. In this paper, a complimentary large-scale view is presented. Extratropical cyclones have been previously shown to affect satellite-retrieved aerosol optical depth (τ), due to enhanced emission of sea salt and sea surface brightness artefacts in regions of higher wind speed. Extratropical cyclones have also been shown to affect cloud-related properties such as cloud fraction (<i>f</i><sub>c</sub>) and cloud top temperature (<i>T</i><sub>top</sub>). Therefore, it seems plausible to hypothesise that extratropical cyclones may drive relationships between cloud-related properties and τ. In this paper, this hypothesis is investigated for extratropical cyclones, henceforth referred to as storms, over the Atlantic Ocean. MODerate resolution Imaging Spectroradiometer (MODIS) retrieved τ, <i>f</i><sub>c</sub> and <i>T</i><sub>top</sub> data are analysed using a storm-centric coordinate system centred on extratropical cyclones which have been tracked using European Centre for Medium Range Weather Forecasts (ECMWF) reanalysis 850 hPa relative vorticity data. The tracked relative vorticity (ω) is used as a measure of storm strength, while position in the storm-centric domain is used to account for storm structure. Relationships between the cloud-related properties and τ are measured by calculating regression slopes and correlations. The <i>f</i><sub>c</sub>–τ relationships are positive, while the <i>T</i><sub>top</sub>–τ relationships are negative. By shuffling the pairing of the cloud and τ data at each location in the storm-centric domain and within narrow ω bins, the contribution of storm strength and storm structure to the observed relationships can be investigated. It is found that storm strength and storm structure can explain only a small component of the relationships observed in the MODIS data. The primary causes for observed cloud–aerosol relationships are likely to be other factors such as retrieval errors, local meteorology or aerosol–cloud interactions.
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An air parcel model was developed to study the formation of small convective clouds that appear under conditions of weak updraft and a strong thermal inversion layer above the clouds. Observations suggest that these clouds are characterized by a cloud base height far lower than the lifting condensation level. Considering such atmospheric conditions, the air parcel model shows that these clouds cannot be the result of classical thermals or plumes that are caused by perturbations in the temperature near the surface. We suggest that such clouds are the result of perturbations in the relative humidity of elevated air pockets. These results explain the existence of small clouds that standard methods fail to predict and shed light on processes related to the formation of convective clouds from the lowest end of the size distribution.
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We report results from two pairs of chemistry-climate model simulations using the same climate model but different chemical perturbations. In each pair of experiments an ozone change was triggered by a simple change in the chemistry. One pair of model experiments looked at the impact of polar stratospheric clouds (PSCs) and the other pair at the impact of short-lived halogenated species on composition and circulation. The model response is complex with both positive and negative changes in ozone concentration, depending on location. These changes result from coupling between composition, temperature and circulation. Even though the causes of the modelled ozone changes are different, the high latitude Southern Hemisphere response in the lower stratosphere is similar. In both pairs of experiments the high-latitude circulation changes, as evidenced by N<sub>2</sub>O differences, are suggesting a slightly longer-lasting/stronger stratospheric descent in runs with higher ozone destruction (a manifestation of a seasonal shift in the circulation). We contrast the idealised model behaviour with interannual variability in ozone and N<sub>2</sub>O as observed by the MIPAS instrument on ENVISAT, highlighting similarities of the modelled climate equilibrium changes to the year 2006–2007 in observations. We conclude that the climate system can respond quite sensitively in its seasonal evolution to small chemical perturbations, that circulation adjustments seen in the model can occur in reality, and that coupled chemistry-climate models allow a better assessment of future ozone and climate change than recent CMIP-type models with prescribed ozone fields.
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A global three-dimensional (i.e. latitude, longitude, altitude) climatology of tropospheric ozone is derived from the ozone sounding record by trajectory mapping. Approximately 52 000 ozonesonde profiles from more than 100 stations worldwide since 1965 are used. The small number of stations results in a sparse geographical distribution. Here, forward and backward trajectory calculations are performed for each sounding to map ozone measurements to a number of other locations, and so to fill in the spatial domain. This is possible because the lifetime of ozone in the troposphere is of the order of weeks. This physically based interpolation method offers obvious advantages over typical statistical interpolation methods. The trajectory-mapped ozone values show reasonable agreement, where they overlap, to the actual soundings, and the patterns produced separately by forward and backward trajectory calculations are similar. Major regional features of the tropospheric ozone distribution are clearly evident in the global maps. An interpolation algorithm based on spherical functions is further used for smoothing and to fill in remaining data gaps. The resulting three-dimensional global tropospheric ozone climatology facilitates visualization and comparison of different years, decades, and seasons, and offers some intriguing insights into the global variation of tropospheric ozone. It will be useful for climate and air quality model initialization and validation, and as an a priori climatology for satellite data retrievals. Further division of the climatology into decadal and annual averages can provide a global view of tropospheric ozone changes, although uncertainties with regard to the performance of older sonde types, as well as more recent variations in operating procedures, need to be taken into account.
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In situ airborne measurements of OH and HO<sub>2</sub> with the HORUS (HydrOxyl Radical measurement Unit based on fluorescence Spectroscopy) instrument were performed in the summertime upper troposphere across Europe during the HOOVER 2 (HO<sub>x</sub> OVer EuRope) campaign in July 2007. Complementary measurements of trace gas species and photolysis frequencies were conducted to obtain a broad data set, which has been used to quantify the significant HO<sub>x</sub> sources and sinks. In this study we compare the in situ measurement of OH and HO<sub>2</sub> with simulated mixing ratios from the constrained box model CAABA/MECCA (Chemistry As A Box Model Application/Module Efficiently Calculating the Chemistry of the Atmosphere), and the global circulation model EMAC (ECHAM5/MESSy Atmospheric Chemistry Model). The constrained box model reproduces the observed OH and HO<sub>2</sub> mixing ratios with better agreement (obs/mod median 98% OH, 96% HO<sub>2</sub>) than the global model (median 76% OH, 59% HO<sub>2</sub>). The observations and the computed HO<sub>x</sub> sources and sinks are used to identify deviations between the models and their impacts on the calculated HO<sub>x</sub> budget.
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This study examines the uncertainties in simulating mass balance and radiative forcing of mineral dust due to biases in the dust size parameterization. Simulations are conducted quasi-globally (180° W–180° E and 60° S–70° N) using the WRF-Chem model with three different approaches to represent dust size distribution (8-bin, 4-bin, and 3-mode). The biases in the 3-mode or 4-bin approaches against a relatively more accurate 8-bin approach in simulating dust mass balance and radiative forcing are identified. Compared to the 8-bin approach, the 4-bin approach simulates similar but coarser size distributions of dust particles in the atmosphere, while the 3-mode approach retains more fine dust particles but fewer coarse dust particles due to its prescribed σ<sub>g</sub> of each mode. Although the 3-mode approach yields up to 10 days of longer dust mass lifetime over the remote oceanic regions than the 8-bin approach, the three size approaches produce a similar dust mass lifetime (3.2 days to 3.5 days) on quasi-global average, reflecting that the global dust mass lifetime is mainly determined by the dust mass lifetime near the dust source regions. <br><br> With the same global dust emission (~4600 Tg yr<sup>−1</sup>), the 8-bin approach produces a dust mass loading of 39 Tg, while the 4-bin and 3-mode approaches produce 3% (40.2 Tg) and 25% (49.1 Tg) higher dust mass loading, respectively. The difference in dust mass loading between the 8-bin approach and the 4-bin or 3-mode approaches has large spatial variations, with generally smaller relative difference (<10%) near the surface over the dust source regions. The three size approaches also result in significantly different dry and wet deposition fluxes and number concentrations of dust. The difference in dust aerosol optical depth (AOD) (a factor of 3) among the three size approaches is much larger than their difference (25%) in dust mass loading. Compared to the 8-bin approach, the 4-bin approach yields stronger dust absorptivity, while the 3-mode approach yields weaker dust absorptivity. Overall, on quasi-global average, the three size parameterizations result in a significant difference of a factor of 2~3 in dust surface cooling (−1.02~−2.87 W m<sup>−2</sup>) and atmospheric warming (0.39~0.96 W m<sup>−2</sup>) and in a tremendous difference of a factor of ~10 in dust TOA (top of atmosphere) cooling (−0.24~−2.20 W m<sup>−2</sup>). The impact of different size representations on dust radiative forcing efficiency is smaller. An uncertainty of a factor of 2 is quantified in dust emission estimation due to the different size parameterizations. This study also highlights the uncertainties in modeling dust mass and number loading, deposition fluxes, and radiative forcing resulting from different size parameterizations, and motivates further investigation of the impact of size parameterizations on modeling dust impacts on air quality, climate, and ecosystems.
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Atmospheric aerosols can contain thousands of organic compounds which impact aerosol surface tension, affecting aerosol properties such as heterogeneous reactivity, ice nucleation, and cloud droplet formation. We present new experimental data for the surface tension of complex, reactive organic–inorganic aqueous mixtures mimicking tropospheric aerosols. Each solution contained 2–6 organic compounds, including methylglyoxal, glyoxal, formaldehyde, acetaldehyde, oxalic acid, succinic acid, leucine, alanine, glycine, and serine, with and without ammonium sulfate. We test two semi-empirical surface tension models and find that most reactive, complex, aqueous organic mixtures which do not contain salt are well described by a weighted Szyszkowski–Langmuir (S-L) model which was first presented by Henning et al. (2005). Two approaches for modeling the effects of salt were tested: (1) the Tuckermann approach (an extension of the Henning model with an additional explicit salt term), and (2) a new implicit method proposed here which employs experimental surface tension data obtained for each organic species in the presence of salt used with the Henning model. We recommend the use of method (2) for surface tension modeling of aerosol systems because the Henning model (using data obtained from organic–inorganic systems) and Tuckermann approach provide similar modeling results and goodness-of-fit (χ<sub>2</sub>) values, yet the Henning model is a simpler and more physical approach to modeling the effects of salt, requiring less empirically determined parameters.
